期刊
SURFACE SCIENCE
卷 603, 期 10-12, 页码 1706-1716出版社
ELSEVIER
DOI: 10.1016/j.susc.2008.10.058
关键词
CO-oxidation; Lattice-gas and multiscale modeling; Kinetic Monte Carlo simulation; Fluctuations and reaction fronts
资金
- Division of Chemical Sciences, Office of Basic Energy Sciences of the US Department of Energy (USDOE)
- USDOE Sci-DAC program
- USDOE [DE-AC02-07CH11358]
We describe recent developments in realistic multisite lattice-gas modeling of CO-oxidation on the unreconstructed (100) surfaces of Pd and Rh. Such models must incorporate the following features: multiple adsorption sites for CO; numerous short-ranged repulsive adspecies interactions; very high CO mobility and significant O mobility on the surface; and the appropriate Langmuir-Hinshelwood adsorption-desorption and reaction dynamics and energetics. The preferred binding site for CO depends on the substrate: bridge sites for Pd(100), and on-top sites for Rh(100). These models can address fundamental aspects of behavior for extended single-crystal surfaces: ordering and temperature-programmed-desorption for single-adspecies systems; mixed adlayer ordering and reactive steady-states as well as temperature-programmed-reaction for the two-adspecies reaction system. Such modeling is also effective in analyzing fluctuation effects for CO-oxidation in nanoscale systems, e.g., Field-Emitter-Tips or supported nanoclusters. A separate challenge is to incorporate this type of realistic atomistic-level description into a multiscale treatment of mesoscale spatial pattern formation and reaction front propagation where characteristic lengths are on the order of microns. This can be achieved within a heterogeneous coupled lattice-gas (HCLG) simulation approach which also requires as input a precise treatment of chemical diffusion in the mixed interacting adlayer. (C) 2009 Elsevier B.V. All rights reserved.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据